CN1098328C - Reduction of emissions from FCC regenerators - Google Patents
Reduction of emissions from FCC regenerators Download PDFInfo
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- CN1098328C CN1098328C CN95102565A CN95102565A CN1098328C CN 1098328 C CN1098328 C CN 1098328C CN 95102565 A CN95102565 A CN 95102565A CN 95102565 A CN95102565 A CN 95102565A CN 1098328 C CN1098328 C CN 1098328C
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- 230000009467 reduction Effects 0.000 title claims description 26
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 74
- 238000002485 combustion reaction Methods 0.000 claims abstract description 73
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 69
- 239000001301 oxygen Substances 0.000 claims abstract description 69
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 69
- 239000007789 gas Substances 0.000 claims abstract description 42
- 239000000571 coke Substances 0.000 claims abstract description 26
- 230000002829 reductive effect Effects 0.000 claims abstract description 10
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 66
- 238000000034 method Methods 0.000 claims description 38
- 239000003054 catalyst Substances 0.000 claims description 34
- 229910052757 nitrogen Inorganic materials 0.000 claims description 34
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 28
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 26
- 239000000203 mixture Substances 0.000 claims description 24
- 229930195733 hydrocarbon Natural products 0.000 claims description 20
- 150000002430 hydrocarbons Chemical class 0.000 claims description 20
- 239000004215 Carbon black (E152) Substances 0.000 claims description 19
- 230000008929 regeneration Effects 0.000 claims description 18
- 238000011069 regeneration method Methods 0.000 claims description 18
- 239000002912 waste gas Substances 0.000 claims description 18
- 239000000567 combustion gas Substances 0.000 claims description 17
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 16
- 235000011089 carbon dioxide Nutrition 0.000 claims description 12
- 238000000197 pyrolysis Methods 0.000 claims description 11
- 230000008676 import Effects 0.000 claims description 7
- 238000004939 coking Methods 0.000 claims description 5
- 229910052756 noble gas Inorganic materials 0.000 claims description 5
- 229910021536 Zeolite Inorganic materials 0.000 claims description 4
- 238000006243 chemical reaction Methods 0.000 claims description 4
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 4
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 4
- 239000010457 zeolite Substances 0.000 claims description 4
- 230000001172 regenerating effect Effects 0.000 claims description 2
- 238000009434 installation Methods 0.000 claims 1
- 238000009428 plumbing Methods 0.000 claims 1
- 239000003085 diluting agent Substances 0.000 abstract 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 18
- 229910021529 ammonia Inorganic materials 0.000 description 9
- 230000008569 process Effects 0.000 description 9
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 8
- 230000008859 change Effects 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 5
- 238000005336 cracking Methods 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
- 229910052786 argon Inorganic materials 0.000 description 4
- 229910017464 nitrogen compound Inorganic materials 0.000 description 4
- 150000002830 nitrogen compounds Chemical class 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 238000009826 distribution Methods 0.000 description 3
- 239000008246 gaseous mixture Substances 0.000 description 3
- 239000002699 waste material Substances 0.000 description 3
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 2
- 235000011941 Tilia x europaea Nutrition 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 230000000996 additive effect Effects 0.000 description 2
- 238000007233 catalytic pyrolysis Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- TXKMVPPZCYKFAC-UHFFFAOYSA-N disulfur monoxide Inorganic materials O=S=S TXKMVPPZCYKFAC-UHFFFAOYSA-N 0.000 description 2
- 238000005243 fluidization Methods 0.000 description 2
- 230000014509 gene expression Effects 0.000 description 2
- 239000004571 lime Substances 0.000 description 2
- -1 nitrogenous compound Chemical class 0.000 description 2
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical compound S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- OBOXTJCIIVUZEN-UHFFFAOYSA-N [C].[O] Chemical compound [C].[O] OBOXTJCIIVUZEN-UHFFFAOYSA-N 0.000 description 1
- 239000003570 air Substances 0.000 description 1
- 230000002337 anti-port Effects 0.000 description 1
- 230000027455 binding Effects 0.000 description 1
- 238000009739 binding Methods 0.000 description 1
- 238000010504 bond cleavage reaction Methods 0.000 description 1
- 230000002925 chemical effect Effects 0.000 description 1
- 238000004581 coalescence Methods 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 239000010795 gaseous waste Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000002203 pretreatment Methods 0.000 description 1
- 238000009418 renovation Methods 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 238000004062 sedimentation Methods 0.000 description 1
- 239000002341 toxic gas Substances 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/90—Regeneration or reactivation
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
- C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
- C10G11/182—Regeneration
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/54—Nitrogen compounds
- B01D53/56—Nitrogen oxides
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/40—Ethylene production
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- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Environmental & Geological Engineering (AREA)
- Analytical Chemistry (AREA)
- Materials Engineering (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
- Catalysts (AREA)
- Industrial Gases (AREA)
Abstract
Coke is burned in the regenerator vessel of an FCC complex with a combustion medium consisting of a diluent gas, such as air, enriched with oxygen, The regenerator is operated in partial combustion mode and excess oxygen is introduced into the combustion zone of the regenerator. Emission of nitrogen oxides to the atmosphere is reduced.
Description
The present invention relates to reduce NO in the waste gas
XMethod, relate to the NO that reduces in the catalytic pyrolysis regeneration unit device waste gas specifically
XMethod.
In catalytic pyrolysis process, the riser tube part of hydrocarbon pyrolysis reactor is injected in the hydrocarbon charging, enters riser tube from the catalyst regenerator circulation---and reactor contacts with the catalyzer of heat, just is cracked into lighter, valuable product.When the heat release scission reaction took place, catalyzer was covered by sedimentation of coke.Catalyzer and hydrocarbon steam are promoted to the separate part of reactor, and is separated from one another.Then catalyzer flows into reactor wash-out part, the catalyzer of hydrocarbon entrainment with steam, and by wash-out, the catalyst stream of wash-out enters the catalyst regenerator container through the used catalyst vertical tube by steam jet.
The typical method of catalyst regeneration is that air is imported regenerator vessel, burns the coke on the but catalyzer, and the combustion reactions thermal discharge of coke is very big, so catalyst temperature raises.The activated catalyzer of heat is back to riser tube by regenerated catalyst standpipe again, to finish catalyst recirculation.The waste gas that combustion of coke produces rises to the top of revivifier, leaves away by the revivifier flue.This waste gas contains nitrogen and carbonic acid gas, and generally also contain carbon monoxide, oxygen, sulfur oxide (SO
X), nitrogen oxide (NO
X) and through reducing nitrogenous substances such as the ammonia that generates.
Catalyst regenerator can be operated (operator scheme that has become standard before this type order) by full-burn mode and also can operate by portion C O combustion mode.In the perfect combustion operation, coke perfect combustion on catalyzer becomes CO
2Its exemplary method of operation is to carry out regenerated under the condition that excess of oxygen is provided by excess air.The waste gas of perfect combustion operation mainly comprises CO
2, nitrogen and superfluous oxygen, but also contain NO
XAnd SO
X
In the operation of part CO burning pattern, air capacity used during the catalyst regenerator operation is for the whole coke in the catalyzer are burnt into CO
2Be insufficient, generate CO and CO so coke just burns
2Mixture.CO wherein is oxidized to CO in a CO burning boiler in downstream
2, the air-flow that comes out of CO boiler contains and is mainly CO thus
2And nitrogen, but also contain NO
XAnd SO
X
Recently, people are to the NO of refinery flares to environment release
XAnd SO
XVery pay close attention to.The view of accepting with regard to these people is the most of NO that is present in catalyst regenerator waste gas
XBe from heterogeneous ring compound, for example, there is the nitrogen in the coke in the condensed cyclic cpds, and the NO in the waste gas
XSeldom or not produce from the airborne nitrogen of regenerator feed.Nitrogen in the coke changes NO into
XMechanism be different, depend on that specifically revivifier is to operate by full-burn mode or by the partial combustion pattern.In the revivifier operation of full-burn mode, the nitrogen in the coke changes NO into
XMixture with elemental nitrogen.In this operator scheme, when the concentration of excess of oxygen in the revivifier increases, NO in the catalyst regenerator waste gas
XAmount also super in increase.
When revivifier is operated by portion C O combustion mode, the NO that in revivifier, produces
XSeldom, the form that contains ammoniacal substance that the ammonia in the coke generates with reduction, for example ammonia leaves revivifier.The ammoniacal substance that this reduction generates is unsteady in the CO boiler, changes NO easily into
XAnd elemental nitrogen.
In order to reduce NO in the catalyst for cracking regenerator off-gas
XContent, the industrial several measures of having taked.The very expensive way of investment is arranged in these measures, for example, reactor feed is carried out the aftertreatment of pre-treatment and waste gas with hydrogen; The medium way of cost is also arranged, for example, hydrocarbon reaction is taked to shunt injecting feeding; Expensive more cheap way is also arranged, for example, adopt catalyzer and catalyst additive.
Minimizing is by NO in the unitary boiler exhaust pipe that is in the downstream of the FCC of fractional combustion pattern operation
XEffort, all be to concentrate on to manage to reduce ammonia and other NO in the regenerator off-gas
XThe content of precursor.United States Patent (USP) 4755282 has disclosed the content that the precious metal that adopts on a kind of inorganic carrier reduces ammonia in the regenerator off-gas.United States Patent (USP) 4744962 has disclosed in the exhaust pipeline to revivifier or downstream and has added NO
XWay.5021144 of United States Patent (USP)s have disclosed and have added the way that revivifier that excessive CO promotor reduces portion C O combustion mode operation is chosen ammonia in the gas.
United States Patent (USP) 5268089 is pointed out, if so-called " edge " pattern is adopted in the operation of revivifier, promptly its operator scheme (this moment, excessive CO was less than 0.05 mole of %) between common portion C O combustion mode and full-burn mode can reduce NO
XContent.This patent is also pointed out, during with this pattern operation, the ammoniate that the reduction that forms in the operation of portion C O combustion mode generates, for example ammonia can be oxidized to nitrogen oxide and elemental nitrogen, and because of dominant reducing environment in revivifier, nitrogen oxide was reduced into elemental nitrogen again before leaving revivifier.Operate with above-mentioned pattern, shortcoming is that regenerator temperature is very high, and the afterfire phenomenon can occur, just not saying the difficulty of revivifier controllability.
Have several patents to disclose by promotor, the means such as aftertreatment of shunting charging cracking, waste gas reduce NO in the FCC revivifier
XContent.These patents go through in United States Patent (USP) 5268089, and are incorporated among the present invention by reference.Owing to oppose the immense pressure of atmosphere toxic gas consequence from environment protection scholar and other personage, people in constantly striving to find new and improved minimizing industrial gaseous waste for example, NO in the FCC regenerator off-gas
XAnd SO
XMethod.The present invention utilizes portion C O
XThe regional rich oxygen containing measure selected in the revivifier that makes is adopted in special nitrogen chemical effect in the combustion mode, reduction ejecta NO
XMethod.
Process of the present invention is exactly to regenerate for the hydrocarbon processing catalyzer of coking, it is at the last one oxidation zone middle part and the most of coke on burning-off catalyzer under the partial combustion condition, nitrogen transformation in the coke of near small part is a nitrogen oxide thus, and then nitrogen oxide the last one reduction zone of flowing through is changeed and to be elemental nitrogen again.
First simultaneously also more general embodiment of the present invention, be exactly to contact (wherein oxygen concn at least about 24% volume) in a combustion zone with the mixture of oxygen and rare gas element from the coked catalyst of hydrocarbon processing devices, the temperature during contact most coke of make suring burns into the mixture of carbon monoxide and carbonic acid gas, this moment and the oxide compound that will be oxidized to basically from the nitrogenous compound that generates through reduction of coke.The total amount of oxygen in the combustion zone just makes these combustion gases that leave the combustion zone contain the carbon monoxide of about 1% (volume).The combustion gases that come out by the combustion zone pass through a reduction zone again, will make nitrogen oxide be reduced to no plain nitrogen herein.
The gas that enters the combustion zone contains aerobic and one or more rare gas elementes, such as nitrogen, argon, carbonic acid gas or their mixture.Enter the typical this feed gas mixtures of combustion zone, can be the mixture of mixture, oxygen and argon of air, oxygen-rich air, oxygen and carbon monoxide and the mixture of oxygen-rich air and carbon monoxide.Preferable gaseous mixture can be with the gaseous mixture of oxygen-rich air or oxygen and carbon dioxide, and oxygen level wherein is at least about 25.5% (volume).What enter oxygen in the gaseous mixture of combustion zone generally must make in the combustion zone the about 650-815 of dominant temperature ℃ in concentration, make about 670-790 ℃ better.
This scheme specifically is applicable to the regeneration of hydrocarbon pyrolysis catalyzer, the hydrocarbon pyrolysis catalyzer of the fluidized-bed form of especially regenerating.
In the preferred versions of invention, combustion zone and reduction zone all are positioned among the catalyst regeneration vessel.Best bet is the lower curtate that the combustion zone is positioned at regeneration container, and the reduction zone is positioned at the top of regeneration container, promptly is positioned at the top, combustion zone.In fact, described reduction zone is positioned at the downstream of described combustion zone.
In one embodiment of the invention, all gases that enter the combustion zone mixes earlier, enters the combustion zone then.In another preferable embodiment, these gases are with two strands or multiply air-flow importing combustion zone.In one situation of back, first gas stream that contains aerobic and rare gas element import the combustion zone than lower part, second gas stream of oxygen or oxygen one noble gas mixtures then imports the combustion zone part that is positioned at the first gas stream entry site downstream.At this moment, best way is that first gas stream is air, oxygen-rich air or oxygen one carbon dioxide gas mixture, and second gas stream is oxygen-rich air or high pure air.
Before address, the amount that imports the oxygen of combustion zone should make and contain about 1% carbon monoxide at least in combustion gases, it is better to contain about 3% carbon monoxide at least, to make combustion gases contain at least 3.5% carbon monoxide be best and be restricted to.
In preferable embodiment of the present invention, this renovation process has constituted a part of FCC operating process, this FCC operating process promptly is that the regenerated catalyst of heat is transferred to hydrocarbon pyrolysis reactor by catalyst regenerator, contact with fresh hydrocarbon therein, make its cracking become the hydrocarbons of lower molecular weight, in this process, just deposited coke on the catalyzer gradually.With the catalyzer of this coking with cracking hydrocarbon be back in the revivifier again after separating and regenerate.
In two embodiments of equipment used, the present invention adopts a fluidisation bed catalyst revivifier, and it has a combustion zone, a reduction zone and two or more import oxygen-containing gas the e Foerderanlage of combustion zone.In a preferable embodiment, one in these e Foerderanlages is the bottom that is positioned at the combustion zone, and second people's e Foerderanlage is positioned at the top of first e Foerderanlage, the top of preferably close combustion zone.
In the embodiment of equipment, a more excellent way is to comprise a device that contained carbon monoxide in the combustion exhaust is further burnt into carbonic acid gas in the device systems.
Fig. 1, the sectional view 1 of a catalyst regenerator of FCC apparatus, it illustrates one embodiment of the invention.
Fig. 2, the another sectional view of catalyst regenerator shown in Figure 1, it illustrates a preferable embodiment of the present invention.
Fig. 3 is the view along the top oxygen-containing gas device of Fig. 1 center line 11-11 line.
Fig. 4 is the enlarged view of combustion zone shown in Figure 2.
The invention provides a kind of method that can reduce content of nitrogen oxide in the FCC catalyst regeneration device institute waste discharge gas considerably.Be present in Jiao on the catalyzer, the oxygen that usually 20.9% (volume) oxygen level of concentration is higher in using than air in the combustion zone of revivifier and the mixture burns of rare gas element are removed employing.This combustion atmosphere can reduce nitrogen in the coke and change the nitrogen compound that reduction generates into.The amount of ammonia for example, and the nitrogen that increases among Jiao produces the amount of the oxidation of nitrogen in the combustion zone.The total amount of oxygen is limited in the combustion zone, so revivifier is by partially combusted pattern work.Thereby the waste gas that leaves the combustion zone contains enough carbon monoxide and produces a reduction zone in the downstream, combustion zone, and consequently nitrogen oxide is reduced into harmless elemental nitrogen.
There is reducing atmosphere to exist in the downstream of combustion zone, most important to the success of the present invention's operation.That is to say, when revivifier by partial combustion pattern operation, and leave when having at least 1% carbon monoxide in the waste gas of combustion zone of revivifier, result of the present invention must be exactly in the burning gas nitrogen oxide be reduced.In addition, for the nitrogen compound that promotes burnt reduction to generate virtually completely is transformed into nitrogen oxide partial oxygen enrichment zone (being the combustion zone), oxygen in the combustion zone must be at least 24 moles of %, and in entering the argon body of combustion zone, oxygen level is preferably 25.5 moles of %.
Change into the amount of nitrogen oxide and nitrogen in regular turn for the nitrogen compound that improves part reduction generation, and the nitrogen oxide that improves generation is reduced into the amount of elemental nitrogen simultaneously, revivifier should be operated about 650-815 ℃ temperature range, and is better about 670-790 ℃ temperature range.
In a preferable embodiment of the present invention, auxiliary oxygen high slightly position on main combustion gases system of distribution is introduced in the bed.So guaranteed that the nitrogenous substances that reduction generates is transformed into oxynitride, and nitrogen oxide finally was reduced during by above-mentioned pattern operation before leaving revivifier.
In the operation of portion C O combustion mode, with enriching antiport to the minimum part of temperature in a large number.Known that under the operational condition of " standard " (perfect combustion) pattern increase excess of oxygen content, amount of nitrogen oxides increases.With the revivifier reducible nitrogen oxide compound of oxygen coalescence, this point may seem and intuition is conflicted.Yet the operation that is applied to portion C O combustion mode can not be directly indiscriminately imitated in this reasoning, in the case, and the main source of oxynitride in the boiler in downstream.Certainly people can not believe, adopt enriched air By that the quantity discharged of the oxynitride in the regenerator off-gas is reduced for the single-stage regeneration device by the full-burn mode operation.
Simultaneously, in revivifier, there is the oxygen of high level to exist, will strengthens taking off SO
2The effect of affixture is because these take off SO
XThe SO that in revivifier, draws of additive
XBe SO3 rather than SO
2Removing SO in the device again
XMany more, then hydrogen sulfide is many more in the catalyzer reactor product of discharging, and the latter can reclaim with several known methods.
Description of drawings the catalyst regenerator that had of FCC system, they can be in order to realize aforesaid several embodiment of the present invention.Also comprised various pipelines among the figure, purpose is in order to explain several aspect of the present invention.For simplicity, hydrocarbon pyrolysis reactor and auxiliary process equipment, valve, instrument etc., because directly do not relate to the present invention, and to understanding the present invention, and inessential so all omit in the drawings.In each figure, identical or similar parts are all represented with identical numbering.
Refer now to the embodiment of representing among Fig. 1 and Fig. 2.Used catalyst transfer lime 4, regenerated catalyst 6, oxygen-containing gas air-supply duct 8, waste pipe 10 are equipped with in the outside of hydrocarbon pyrolysis catalyst regenerator 2.The combustion zone is generally with 12 expressions, and the reduction zone is generally with 14 expressions, and they lay respectively at the low and higher position of revivifier 2 inside.Inlet pipe 16 links the central authorities of air-supply duct 8 to sparger 18.Nozzle 20 is housed on the sparger 18.Among diagram 20 embodiments, sparger 18 is two mutually perpendicular arms that level is arranged in revivifier 2 lower positions; Yet sparger 18 can have any required structure, for example can be the circular ring type pipe of extended loop around revivifier 2.Described catalyzer is selected from X type zeolite, y-type zeolite and composition thereof.
Combustion zone 12 is burnt incendiary zones that take place in the revivifier 2.Because generation when burning is that the coke of heat contacts with oxygen is so the scope of combustion zone 18 is just limited by the oxygen that enters revivifier 1.In the equipment shown in Fig. 1, nozzle 10 is installed down, the below of the sparger 18 that oxygen-containing gas can be led, and the result has just enlarged the scope of combustion zone 11.
Waste pipe 10 is with the top of revivifier 2 and an optional CO (carbon monoxide converter) boiler 12 bindings.Boiler 22 runs at its exit end and puts pipe 24.If without CO (carbon monoxide converter) boiler, the waste gas of carbon monoxide is just transported to next operation steps and is made step processing, for example conversion reaction.
In system operation process illustrated in figures 1 and 2, from hydrocarbon pyrolysis reactor (not shown) with exhausted hydrocarbon pyrolysis catalyzer.By used catalyst transfer lime 4 input revivifiers 2.
At this moment, the used catalyst of input is made tangential motion around the inside of revivifier 2.Like this, formed the dilute phase fludization bed, formed the dense-phase fluidization bed at the position down of revivifier with regard to the top of revivifier 2.When catalyzer contacts with oxygen one in the air inlet, Jiao on the catalyst surface gets up with fire burns, produces to contain carbonic acid gas, carbon monoxide, water vapor, nitrogen oxide, may also contain the combustion gases of sulfur oxide.
The total oxygen level that enters the gas of revivifier 2 is not so that all coke are transformed into carbonic acid gas, and promptly revivifier 2 is by the work of partial combustion pattern.Yet reductive nitrogen all is transformed into nitrogen oxide basically in the coke compound for making, and the oxygen in the air inlet still is enough.If oxygen level is less in the air inlet, the part of nitrogen will change the compound that nitrogen generates for reduction in the coke.For example, ammonia.This compounds will change nitrogen oxide in the high oxidation atmosphere of the CO (carbon monoxide converter) boiler that is arranged in revivifier 2 downstreams.
Combustion gases rise to the top of revivifier 2 apace, just enter reduction zone 4, and an oxygen carbon concentration is enough high so this district is a reduction atmosphere in this district.When waste gas during through reduction zone 14, nitrogen oxide or its major part all change elemental nitrogen into.Then combustion gases enter CO (carbon monoxide converter) boiler 22 (if adopting this equipment in system).Waste gas leaves boiler 22, and this moment, it was essentially carbonic acid gas, may also have nitrogen, discharges by vapor pipe 24.When gas passed through boiler 22, the carbon monoxide in waste gas changed carbonic acid gas into, but the then rare further oxidation of the nitrogen in the waste gas.So by method of the present invention, the nitrogen compound that a little reduction of base generate will be changed into more stable elemental nitrogen, and without the inventive method, they can become nitrogen oxide.Fig. 3 and Fig. 4 have represented a preferable embodiment of the present invention.In this scheme, auxiliary oxygen distribution device 26 is positioned at the top of oxygen distribution device 18, the top 12a of burner.Sparger 26 is connected to oxygen supply pipe 28 and nozzle 30.
In the operation of the inventive method embodiment of Fig. 3 and Fig. 4, used catalyst still enters revivifier 2 in above-mentioned mode.Enter revivifier 2 by inlet pipe 16 oxygen-containing gass.This gas is a kind of oxygen one noble gas mixtures.It can be an air, oxygen-rich air, the mixture of oxygen one carbonic acid gas or oxygen and other rare gas element.For example, oxygen one argon gas body mixture or oxygen-rich air---carbon dioxide gas mixture.
By oxygen supply pipe 28, sparger 26 and nozzle 30, with another feed importing combustion zone 12a of oxygen-containing gas.This gas can be exactly pure oxygen basically, promptly contains the oxygen of other gas no more than 1%; Perhaps high purity oxygen promptly contains at least about 80%, and the preferable gas that contains at least 90% oxygen; Or oxygen-rich air.With the purpose of this gas, be the oxidation atmosphere of overheavy firing district 12a by sparger 26 feeding combustion zones.Can guarantee that thus the nitrogen among Jiao is converted into the intermediate nitrogen oxide more completely, thereby be converted into elemental nitrogen again after guaranteeing.Leave the combustion gases of combustion zone 12a, just by reduction zone 14 and the CO (carbon monoxide converter) boiler 22 that can add use as mentioned above.
Should be appreciated that, adopt conventional equipment air-flow in the system to be monitored and regulate automatically and make its fully automated, make process continuous operation effectively, also belong to scope of the present invention.
Although the present invention is illustrated by a particular experiment example, the present invention that has been illustration only of this example can have and change expection.For example, method of the present invention can be implemented in being different from the equipment arrangement shown in the figure, and the present invention can be applied to the system different with the FCC system, for example fixed bed system.The restriction that scope of the present invention is limited by appended claims only.
Claims (19)
1. one kind makes the hydrocarbon pyrolysis catalyzer with deposits of coke carry out the regenerated method by this deposits of coke of burning, and it is characterized in that comprising the following steps:
(a) described catalyzer is contacted in medial temperature 650-815 ℃ combustion zone with oxygen one noble gas mixtures, the composition of oxygen in described mixture that imports described combustion zone accounts for 24% at least, burn described coke thus to small part, and the nitrogen in described coke is transformed into nitrogen oxide, and the result produces the combustion gases of the anaerobic basically of carbonated, nitrogen oxide and at least 1% carbon monoxide;
(b) with described combustion gases by a reduction zone, be transformed into elemental nitrogen to the described nitrogen oxide of small part thus.
2. the method for claim 1 is characterized in that described catalyst bed is fluidized state.
3. method as claimed in claim 2 is characterized in that, described combustion zone and described reduction zone all are arranged in a catalyst regeneration vessel.
4. method as claimed in claim 3 is characterized in that, described combustion zone be positioned at described regeneration container than lower part and described reduced zone is positioned at the downstream of described combustion zone.
5. method as claimed in claim 4 is characterized in that, described catalyzer circulates between described regeneration container and hydrocarbon pyrolysis reaction vessel.
6. method as claimed in claim 5 is characterized in that, described catalyzer is selected from X type zeolite, y-type zeolite and composition thereof.
7. the method for claim 1 is characterized in that, described oxygen-noble gas mixtures contains aerobic and a kind of gas that is selected from nitrogen, carbonic acid gas and composition thereof.
8. as claim 1 or 7 described methods, it is characterized in that described combustion gases contain 3% carbon monoxide at least.
9. as claim 1 or 7 described methods, it is characterized in that described oxygen-noble gas mixtures contains 25.5% oxygen at least.
10. as claim 1 or 7 described methods, it is characterized in that oxygen imports described combustion zone at least in two strands of feed streams.
11. method as claimed in claim 10 is characterized in that, described combustion gases contain 3.5% carbon monoxide at least.
12. method as claimed in claim 10 is characterized in that, one feed stream is air or oxygen-rich air.
13. method as claimed in claim 10 is characterized in that, one feed stream is oxygen-rich air or pure basically oxygen.
14. method as claimed in claim 13 is characterized in that, described one feed stream that imports described regeneration container enters at one or more of the upper area of described combustion zone.
15. the method for claim 1 is characterized in that, described combustion gases experience a combustion step again, make carbon monoxide all basically in the described waste gas all be transformed into carbonic acid gas.
16. method as claimed in claim 15 is characterized in that, described combustion step carries out in CO (carbon monoxide converter) boiler.
17. method as claimed in claim 15 is characterized in that, is transformed into carbonic acid gas by water-gas shift reaction to the small part carbon monoxide in described combustion gases.
18. the equipment of the hydrocarbon pyrolysis catalyzer of the coking of regenerating is characterized in that it comprises:
(a) catalyst regeneration vessel;
(b) catalyzer of coking is introduced the pipeline of described revivifier and keep the catalyzer of described coking in described revivifier, to be the device of fluidized;
(c) a kind of oxygen-containing gas is introduced the device of first in the described regeneration container Lower Half;
(d) a kind of oxygen-containing gas is introduced the device of second in the described regeneration container Lower Half, but the position of its introducing is higher than the position that first device is introduced;
(e) be positioned at described first below of installing, be used for from described regeneration container, removing the plumbing installation of regenerated catalyst; And
(f) be positioned at described second top of installing, be used for from described regeneration container, removing the device of combustion gases;
19. device as claimed in claim 18 is characterized in that, it comprises that further the carbon monoxide in the combustion gases that will remove carries out the incendiary device from described regeneration container.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US31565694A | 1994-09-30 | 1994-09-30 | |
| US08/315,656 | 1994-09-30 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1126238A CN1126238A (en) | 1996-07-10 |
| CN1098328C true CN1098328C (en) | 2003-01-08 |
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|---|---|---|---|
| CN95102565A Expired - Fee Related CN1098328C (en) | 1994-09-30 | 1995-09-28 | Reduction of emissions from FCC regenerators |
Country Status (16)
| Country | Link |
|---|---|
| US (1) | US5908804A (en) |
| EP (1) | EP0704516B1 (en) |
| JP (1) | JP3913281B2 (en) |
| KR (1) | KR100191974B1 (en) |
| CN (1) | CN1098328C (en) |
| AU (1) | AU688571B2 (en) |
| CA (1) | CA2156464C (en) |
| DE (1) | DE69529196T2 (en) |
| ES (1) | ES2184783T3 (en) |
| MY (1) | MY113199A (en) |
| NO (1) | NO313793B1 (en) |
| NZ (1) | NZ272844A (en) |
| PL (1) | PL179607B1 (en) |
| TR (1) | TR199501185A2 (en) |
| TW (1) | TW350871B (en) |
| ZA (1) | ZA957448B (en) |
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| US6491810B1 (en) | 2000-11-01 | 2002-12-10 | Warden W. Mayes, Jr. | Method of producing synthesis gas from a regeneration of spent cracking catalyst |
| US6916417B2 (en) * | 2000-11-01 | 2005-07-12 | Warden W. Mayes, Jr. | Catalytic cracking of a residuum feedstock to produce lower molecular weight gaseous products |
| US6579820B2 (en) | 2001-03-21 | 2003-06-17 | The Boc Group, Inc. | Reactor modifications for NOx reduction from a fluid catalytic cracking regeneration vessel |
| US6505567B1 (en) * | 2001-11-26 | 2003-01-14 | Alstom (Switzerland) Ltd | Oxygen fired circulating fluidized bed steam generator |
| ATE329985T1 (en) * | 2002-03-27 | 2006-07-15 | Shell Int Research | METHOD FOR COMBUSTION OF COKE DURING REGENERATION OF AN FCC CATALYST. |
| US7026262B1 (en) * | 2002-09-17 | 2006-04-11 | Uop Llc | Apparatus and process for regenerating catalyst |
| US20040074809A1 (en) * | 2002-10-21 | 2004-04-22 | George Yaluris | Reduction of gas phase reduced nitrogen species in partial burn FCC processes |
| US20040262197A1 (en) * | 2003-06-24 | 2004-12-30 | Mcgregor Duane R. | Reduction of NOx in low CO partial-burn operation using full burn regenerator additives |
| US20050100494A1 (en) | 2003-11-06 | 2005-05-12 | George Yaluris | Ferrierite compositions for reducing NOx emissions during fluid catalytic cracking |
| US20050100493A1 (en) * | 2003-11-06 | 2005-05-12 | George Yaluris | Ferrierite compositions for reducing NOx emissions during fluid catalytic cracking |
| WO2005060519A2 (en) * | 2003-12-05 | 2005-07-07 | Intercat, Inc. | Mixed metal oxide sorbents |
| US7304011B2 (en) * | 2004-04-15 | 2007-12-04 | W.R. Grace & Co. -Conn. | Compositions and processes for reducing NOx emissions during fluid catalytic cracking |
| US20050232839A1 (en) * | 2004-04-15 | 2005-10-20 | George Yaluris | Compositions and processes for reducing NOx emissions during fluid catalytic cracking |
| ITBO20040296A1 (en) * | 2004-05-11 | 2004-08-11 | Itea Spa | High efficiency and reduced environmental impact combustors, and processes for the production of electricity deriving from it |
| JP5383184B2 (en) | 2005-04-27 | 2014-01-08 | ダブリュー・アール・グレイス・アンド・カンパニー−コネチカット | Compositions and methods for reducing NOx emissions during fluid catalytic cracking |
| US7470412B2 (en) * | 2005-12-21 | 2008-12-30 | Praxair Technology, Inc. | Reduction of CO and NOx in regenerator flue gas |
| KR100824763B1 (en) * | 2006-09-25 | 2008-04-24 | 희성촉매 주식회사 | A method for regenerating catalysts |
| US7954458B2 (en) * | 2007-11-14 | 2011-06-07 | Alstom Technology Ltd | Boiler having an integrated oxygen producing device |
| US8618012B2 (en) | 2010-04-09 | 2013-12-31 | Kellogg Brown & Root Llc | Systems and methods for regenerating a spent catalyst |
| US8618011B2 (en) | 2010-04-09 | 2013-12-31 | Kellogg Brown & Root Llc | Systems and methods for regenerating a spent catalyst |
| CN102527208B (en) * | 2010-12-30 | 2014-12-31 | 中国石油化工股份有限公司 | Method for removing sulfur oxide and nitrogen oxide in catalytic cracking regenerated smoke |
| JP5660957B2 (en) * | 2011-03-31 | 2015-01-28 | 独立行政法人石油天然ガス・金属鉱物資源機構 | Regenerated hydrocracking catalyst and method for producing hydrocarbon oil |
| JP5660956B2 (en) | 2011-03-31 | 2015-01-28 | 独立行政法人石油天然ガス・金属鉱物資源機構 | Hydrocracking catalyst and method for producing hydrocarbon oil |
| WO2016200566A1 (en) | 2015-06-09 | 2016-12-15 | Exxonmobil Research And Engineering Company | Fluid catalytic cracking unit with low emissions |
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- 1995-09-04 NO NO19953470A patent/NO313793B1/en unknown
- 1995-09-05 ZA ZA957448A patent/ZA957448B/en unknown
- 1995-09-13 EP EP95306405A patent/EP0704516B1/en not_active Revoked
- 1995-09-13 ES ES95306405T patent/ES2184783T3/en not_active Expired - Lifetime
- 1995-09-13 DE DE69529196T patent/DE69529196T2/en not_active Revoked
- 1995-09-14 TW TW084109631A patent/TW350871B/en not_active IP Right Cessation
- 1995-09-15 MY MYPI95002743A patent/MY113199A/en unknown
- 1995-09-27 PL PL95310693A patent/PL179607B1/en not_active IP Right Cessation
- 1995-09-27 AU AU32927/95A patent/AU688571B2/en not_active Ceased
- 1995-09-28 CN CN95102565A patent/CN1098328C/en not_active Expired - Fee Related
- 1995-09-28 JP JP25086895A patent/JP3913281B2/en not_active Expired - Fee Related
- 1995-09-29 TR TR95/01185A patent/TR199501185A2/en unknown
- 1995-09-29 KR KR1019950032875A patent/KR100191974B1/en not_active IP Right Cessation
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Also Published As
| Publication number | Publication date |
|---|---|
| CA2156464C (en) | 1999-07-20 |
| DE69529196T2 (en) | 2003-07-17 |
| KR100191974B1 (en) | 1999-06-15 |
| CA2156464A1 (en) | 1996-03-31 |
| EP0704516B1 (en) | 2002-12-18 |
| PL310693A1 (en) | 1996-04-01 |
| TR199501185A2 (en) | 1996-06-21 |
| NO953470L (en) | 1996-04-01 |
| NO953470D0 (en) | 1995-09-04 |
| ZA957448B (en) | 1996-04-17 |
| ES2184783T3 (en) | 2003-04-16 |
| KR960010080A (en) | 1996-04-20 |
| CN1126238A (en) | 1996-07-10 |
| AU688571B2 (en) | 1998-03-12 |
| AU3292795A (en) | 1996-04-18 |
| PL179607B1 (en) | 2000-10-31 |
| NZ272844A (en) | 1997-05-26 |
| DE69529196D1 (en) | 2003-01-30 |
| JP3913281B2 (en) | 2007-05-09 |
| NO313793B1 (en) | 2002-12-02 |
| EP0704516A2 (en) | 1996-04-03 |
| EP0704516A3 (en) | 1996-05-08 |
| TW350871B (en) | 1999-01-21 |
| MY113199A (en) | 2001-12-31 |
| JPH08173817A (en) | 1996-07-09 |
| US5908804A (en) | 1999-06-01 |
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